Spinel structured LTO (lithium titanium oxide), Li4Ti5O12, materials have gained renewed interest in electrodes for lithium-ion batteries. Powder precursors were mixed by HEBM (high energy-ball mill) and Li4Ti5O12 was formed by calcinations at high temperature. The influence of excess Li on the structural characteristics of lithium titanium oxide was investigated. According to the XRD and SEM analysis, uniformly distributed Li4Ti5O12 particles were synthesized. Li4Ti5O12 had different characteristics due to the precursor sizes and the heat treatment temperatures. LTO from micro TiO2 showed the highest discharge capacity at 750 oC for 12 h. LTO from nano TiO2 showed the highest discharge capacity at 700 ℃ for 12 h. Lithium-ion battery with Li4Ti5O12 anode and lithium metal cathode showed the capacity of 170 mAh/g at 1.0-3.0 V.